Mn-MCM-41 Türü Katalizörler ile Model Atıksulardan Fenol Giderimi

Bu çalışma kapsamında farklı Mn/Si molar oranlarında, Mn katkılı MCM-41 katalizörleri sentezlenmiş ve katalizörlerin karakterizasyonu, XRD, BET, SEM, EDS ve parçacık boyut analizi metotları kullanılarak yapılmıştır. Katalizörlerin aktiviteleri, hidrojen peroksit katkılı yaş katalitik oksidasyon ile model atık sulardan fenol giderimi tepkimesinde test edilmiştir. XRD ve BET sonuçları, saf silikat formdaki MCM-41 destek malzemesinin istenilen altıgen gözenekli yapıda olduğunu, manganez metali eklendiğinde ise kristal yapının bozularak amorf yapıya dönüştüğünü, gözeneklerin kısmen bloke olması nedeniyle de BET yüzey alanlarının önemli ölçüde azaldığını göstermiştir. Fenol giderim reaksiyonları, laboratuar ortamında hazırlanan 50 ppm’lik fenol çözeltisi kullanılarak, 25,40 ve 60oC’de, 6,0 olarak ölçülen başlangıç pH’sında ve kesikli reaktörde yürütülmüştür. Deney sonuçları, optimum metal yüklemesinin Mn/Si molar oranı 0,06 olduğunda gerçekleştiğini göstermiştir. Reaksiyon bulguları incelendiğinde, sıcaklıkla birlikte fenol gideriminin arttığı görülmüştür. Buna ek olarak, atmosferik basınç ve çalışılan farklı sıcaklıklarda, katalizör yapısına metal eklenmesiyle birlikte fenol gideriminin, saf silika yapısındaki MCM-41’e oranla, Mn-MCM-41 katalizörleri için, %4.6-%14.4 aralığında arttığı görülmüştür. Optimum reaksiyon koşulları, atmosferik basınç, 60oC, 0,06 Mn/Si molar oranı olarak tespit edilmiş ve bu koşullarda %56 fenol giderimi elde edilmiştir. Ilımlı tepkime koşullarında (60oC ve atmosferik basınç), az miktarda metal ve az miktarda katalizör kullanarak (Mn/Si molar oranı 0,060, katalizör miktarı1,0 g/L), Mn-MCM-41 katalizörleri ile orta derece konsantre model atıksulardan optimum %56 fenol giderimi elde edilmesinin literatüre önemli bir katkı sağlayacağı düşünülmektedir.

Anahtar Kelimeler:

Mn-MCM-41, Fenol, Atık su

Phenol Removal From Model Waste Waters by Mn-MCM-41 Type Catalysts

In this study, Mn-incorporated MCM-41 catalysts with different Mn/Si molar ratios were synthesised and the characterisation of the catalysts was carried out by using XRD, BET, SEM, EDS and particle size analysis methods. The activities of the catalysts were tested in the phenol removal reaction from model solutions using the wet catalytic oxidation with hydrogen peroxide. XRD and BET results showed that the MCM-41 support material in the pure silicate form had the desired hexagonal porous structure but upon addition of the manganese metal, the crystal structure deteriorated becoming amorphous and the surface areas reduced significantly due to the partial blocking of the pores. Phenol removal reactions were carried out using a 50 ppm phenol solution prepared in the laboratory at 25,40 and 60oC, at an initial pH value of 6.0 in a batch reactor. The experimental results depicted that the optimum metal loading occurred at a Mn/Si molar ratio of 0.06. Investigation of the reaction results showed that phenol removal increased with temperature. In addition, at atmospheric pressure and at the studied different temperatures, with the addition of the metal to the MCM-41 structure, the phenol removal percentage increased in the range of 4.6%-14.4% for Mn-MCM-41 catalysts, compared to the purely siliceous MCM-41. Optimum reaction conditions were determined as 60oC, atmospheric pressure, 0.06 Mn/Si molar ratio, and 56% phenol removal was obtained under these conditions. Obtaining an optimum 56% phenol removal from moderately concentrated model waste waters with Mn-MCM-41 catalysts by using a small amount of metal and small amount of catalyst (Mn/Si molar ratio 0.060, catalyst amount 1.0 g/L) under moderate reaction conditions (60oC and atmospheric pressure), is thought to make an important contribution to the literature.

Keywords:

Mn-MCM-41, Phenol, Wastewater,

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